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Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies
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Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies

A special issue of Applied Sciences (ISSN 2076-3417). This special issue belongs to the section "Chemical and Molecular Sciences".

Deadline for manuscript submissions: closed (30 June 2020) | Viewed by 63789

Printed Edition Available!
A printed edition of this Special Issue is available here.

Special Issue Editors

Dr. Nikolaos Koukouzas

E-Mail Website
Guest Editor
Chemical Process & Energy Resources Institute, Centre for Research & Technology Hellas (CERTH),15125 Athens, Greece
Interests: energy storage and policy; hydrogen; carbon capture and stotage; geo-engineering; hydro-pump energy storage; nanomaterials; land reclamation; ultramafic rocks petrology; industrial minerals; critical raw materials
Special Issues, Collections and Topics in MDPI journals
Dr. Pavlos Tyrologou

E-Mail Website
Co-Guest Editor
Center for Research & Technology Hellas/Chemical Process and Energy Resources Institute (CERTH/CPERI), 52 Egialias Str., 15125 Maroussi, Athens, Greece
Interests: geological engineering; environmental impact assessment; contaminated land; renewable energy; water resources; climate change; vulnerability; sustainability; fragility; CO2 sequestration
Special Issues, Collections and Topics in MDPI journals
Dr. Petros Koutsovitis

E-Mail Website
Co-Guest Editor
Research Fellow, Centre for Research and Technology Hellas, Chemical Process and Energy Resources Institute (CERTH/CPERI), 52 Egialias str., 15125 Maroussi-Athens, Greece
Interests: petrology; mineralogy; geochemestry; CCUS; reneable energy; energy storage system
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

We are pleased to invite you to contribute an article to an upcoming Special Issue titled: “Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies” which will be published in Applied Sciences Journal. This special issue is open to researchers and authors that want to submit their research and review articles that explore the application of carbon capture and storage technologies, mitigating the effects of climate change. Special emphasis will be given on mineral carbonation techniques. The aim of this issue is to contribute to the knowledge of the ongoing research regarding climate change and CCS technological applications, focusing on carbon capture and storage practices.

Theme of the Special Issue

Climate change is a global issue that is interrelated with the energy and petroleum industry. In this scope, there is an increasing demand for new low cost and energy efficient techniques that reduce the CO2 emissions. The use of fossil fuels is the primary source of CO2 emissions, which is one of the main greenhouse gases.

Carbon Capture and Storage (CCS) is regarded as one of the most efficient technologies that allows carbon intensive industries to continue to operate with lower CO2 emissions. CCS offers double benefits combining the reduction of greenhouse gas with the direct use of the captured carbon for Enhanced Oil Recovery (EOR). Mineral carbonation is a permanent and secure CCS and sequestration technology that gives the solution in cases of smaller to medium emitters. It is based on the in situ (injecting CO2 into the earth’s surface) or ex situ (chemical reactor systems) production of carbonate minerals through the chemical reaction of CO2 with Ca, Mg and Fe-silicate minerals.

Researchers from the fields of physical sciences and engineering are invited to contribute to our special issue, exchanging the latest research advances in this highly interdisciplinary sector.

Dr. Nikolaos Koukouzas
Dr. Pavlos Tyrologou
Dr. Petros Koutsovitis
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Applied Sciences is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2400 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • climate change
  • CCS
  • CO2-mineralization
  • CO2-utilization

Published Papers (17 papers)

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Editorial

Jump to: Research

3 pages, 183 KiB  
Editorial
Special Issue “Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies”
by Nikolaos Koukouzas, Pavlos Tyrologou and Petros Koutsovitis
Appl. Sci. 2020, 10(21), 7463; https://doi.org/10.3390/app10217463 - 23 Oct 2020
Cited by 1 | Viewed by 1401
Abstract
This Special Issue presents sixteen scientific papers that explore the application of carbon capture and storage technologies, mitigating the effects of climate change [...] Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)

Research

Jump to: Editorial

15 pages, 3730 KiB  
Article
Wettability Alteration by Carbonated Brine Injection and Its Impact on Pore-Scale Multiphase Flow for Carbon Capture and Storage and Enhanced Oil Recovery in a Carbonate Reservoir
by Santiago Drexler, Fernanda Hoerlle, William Godoy, Austin Boyd and Paulo Couto
Appl. Sci. 2020, 10(18), 6496; https://doi.org/10.3390/app10186496 - 17 Sep 2020
Cited by 15 | Viewed by 3514
Abstract
Carbon capture and storage is key for sustainable economic growth. CO2-enhanced oil recovery (EOR) methods are efficient practices to reduce emissions while increasing oil production. Although it has been successfully implemented in carbonate reservoirs, its effect on wettability and multiphase flow [...] Read more.
Carbon capture and storage is key for sustainable economic growth. CO2-enhanced oil recovery (EOR) methods are efficient practices to reduce emissions while increasing oil production. Although it has been successfully implemented in carbonate reservoirs, its effect on wettability and multiphase flow is still a matter of research. This work investigates the wettability alteration by carbonated water injection (CWI) on a coquina carbonate rock analogue of a Pre-salt reservoir, and its consequences in the flow of oil. The rock was characterized by routine petrophysical analysis and nuclear magnetic resonance. Moreover, micro-computed tomography was used to reconstruct the pore volume, capturing the dominant flow structure. Furthermore, wettability was assessed by contact angle measurement (before and after CWI) at reservoir conditions. Finally, pore-scale simulations were performed using the pore network modelling technique. The results showed that CWI altered the wettability of the carbonate rock from neutral to water-wet. In addition, the simulated relative permeability curves presented a shift in the crossover and imbibition endpoint values, indicating an increased flow capacity of oil after CWI. These results suggest that the wettability alteration mechanism contributes to enhancing the production of oil by CWI in this system. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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23 pages, 4223 KiB  
Article
Off-Design Operation of Conventional and Phase-Change CO2 Capture Solvents and Mixtures: A Systematic Assessment Approach
by Theodoros Zarogiannis, Athanasios I. Papadopoulos and Panos Seferlis
Appl. Sci. 2020, 10(15), 5316; https://doi.org/10.3390/app10155316 - 31 Jul 2020
Cited by 4 | Viewed by 2102
Abstract
Solvent-based CO2 capture technologies hold promise for future implementation but conventional solvents incur significant energy penalties and capture costs. Phase-change solvents enable a significant reduction in the regeneration energy but their performance has only been investigated under steady-state operation. In the current [...] Read more.
Solvent-based CO2 capture technologies hold promise for future implementation but conventional solvents incur significant energy penalties and capture costs. Phase-change solvents enable a significant reduction in the regeneration energy but their performance has only been investigated under steady-state operation. In the current work, we employed a systematic approach for the evaluation of conventional solvents and mixtures, as well as phase-change solvents under the influence of disturbances. Sensitivity analysis was used to identify the impact that operating parameter variations and different solvents exert on multiple CO2 capture performance indicators within a wide operating range. The resulting capture process performance was then assessed for each solvent within a multi-criteria approach, which simultaneously accounted for off-design conditions and nominal operation. The considered performance criteria included the regeneration energy, solvent mass flow rate, cost and cyclic capacity, net energy penalty from integration with an upstream power plant, and lost revenue from parasitic losses. The 10 investigated solvents included the phase-change solvents methyl-cyclohexylamine (MCA) and 2-(diethylamino)ethanol/3-(methylamino)propylamine (DEEA/MAPA). We found that the conventional mixture diethanolamine/methyldiethanolamine (DEA/MDEA) and the phase-change solvent DEEA/MAPA exhibited both resilience to disturbances and desirable nominal operation for multiple performance indicators simultaneously. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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24 pages, 6271 KiB  
Article
Mineral Carbonation of CO2 in Mafic Plutonic Rocks, II—Laboratory Experiments on Early-Phase Supercritical CO2‒Brine‒Rock Interactions
by Patrícia Moita, Edgar Berrezueta, Halidi Abdoulghafour, Massimo Beltrame, Jorge Pedro, José Mirão, Catarina Miguel, Cristina Galacho, Fabio Sitzia, Pedro Barrulas and Júlio Carneiro
Appl. Sci. 2020, 10(15), 5083; https://doi.org/10.3390/app10155083 - 23 Jul 2020
Cited by 8 | Viewed by 3066
Abstract
The potential for mineral carbonation of CO2 in plutonic mafic rocks is addressed through a set of laboratory experiments on cumulate gabbro and gabbro-diorite specimens from the Sines Massif (Portugal). The experiments were conducted in an autoclave, for a maximum of 64 [...] Read more.
The potential for mineral carbonation of CO2 in plutonic mafic rocks is addressed through a set of laboratory experiments on cumulate gabbro and gabbro-diorite specimens from the Sines Massif (Portugal). The experiments were conducted in an autoclave, for a maximum of 64 days, using a CO2 supersaturated brine under pressure and temperature conditions similar to those expected around an injection well during early-phase CO2 injection. Multiple techniques for mineralogical and geochemical characterization were applied ante- and post-carbonation experiments. New mineralogical phases (smectite, halite and gypsum), roughness increase and material loss were observed after exposure to the CO2 supersaturated brine. The chemical analysis shows consistent changes in the brine and rock specimens: (i) increases in iron (Fe) and magnesium (Mg) in the aqueous phase and decreases in Fe2O3 and MgO in the specimens; (ii) a decrease in aqueous calcium (Ca) and an increase in CaO in the cumulate gabbro, whereas in the gabbro-diorite aqueous Ca increased and afterwards remained constant, whereas CaO decreased. The geochemical model using the CrunchFlow code was able to reproduce the experimental observations and simulate the chemical behavior for longer times. Overall, the study indicates that the early-stage CO2 injection conditions adopted induce mainly a dissolution phase with mineralogical/textural readjustments on the external area of the samples studied. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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13 pages, 3501 KiB  
Article
Evolutions of CO2 Adsorption and Nanopore Development Characteristics during Coal Structure Deformation
by Linlin Wang and Zhengjiang Long
Appl. Sci. 2020, 10(14), 4997; https://doi.org/10.3390/app10144997 - 21 Jul 2020
Cited by 7 | Viewed by 1824
Abstract
The coal structure deformation attributed to actions of tectonic stresses can change characteristics of nanopore structure of coals, affecting their CO2 adsorption. Three tectonically deformed coals and one undeformed coal were chosen as the research objects. The isotherm adsorption experiments of four [...] Read more.
The coal structure deformation attributed to actions of tectonic stresses can change characteristics of nanopore structure of coals, affecting their CO2 adsorption. Three tectonically deformed coals and one undeformed coal were chosen as the research objects. The isotherm adsorption experiments of four coal specimens were carried out at the temperature of 35 °C and the pressure of 0 to 7 MPa. Nanopore structures were characterized using the liquid nitrogen adsorption method. The results show that there exist maximum values of excess and absolute adsorption capacity, which increase with increasing coal deformation degree. As the degree of coal deformation increases, the pore volume and specific surface area present an obvious increasing trend in the case of micropores, exhibiting an increase at first (cataclastic coal and ganulitic coal) and then stabilization (crumple coal), in the case of mesopores, and showing a gradual decrease in the case of macropores. The mesopores are the key factor of CO2 adsorption of tectonically deformed coals, followed by the micropores and the limited effect of macropores at the strong coal deformation stage. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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19 pages, 16825 KiB  
Article
Mineral Carbonation of CO2 in Mafic Plutonic Rocks, I—Screening Criteria and Application to a Case Study in Southwest Portugal
by Jorge Pedro, António A. Araújo, Patrícia Moita, Massimo Beltrame, Luis Lopes, António Chambel, Edgar Berrezueta and Júlio Carneiro
Appl. Sci. 2020, 10(14), 4879; https://doi.org/10.3390/app10144879 - 16 Jul 2020
Cited by 12 | Viewed by 3189
Abstract
This article describes the screening, ranking and characterization of ultramafic and mafic rocks in southern Portugal for mineral carbonation as an alternative to conventional CO2 storage in sedimentary rocks. A set of criteria including mineralogy, structure, surface area, distance to CO2 [...] Read more.
This article describes the screening, ranking and characterization of ultramafic and mafic rocks in southern Portugal for mineral carbonation as an alternative to conventional CO2 storage in sedimentary rocks. A set of criteria including mineralogy, structure, surface area, distance to CO2 sources, expected volume, and socioeconomic conditions was applied to screen ultramafic and mafic rock massifs in the Alentejo region, southern Portugal. Ranking of the massifs indicated that the plutonic massifs of Sines and of Torrão‒Odivelas were the most promising. A characterization was made of the Sines massif, a subvolcanic massif composed mostly of gabbros and diorites, located immediately adjacent to the CO2 sources and outcropping along 300 km2 onshore and offshore. These studies confirmed that these rock samples exhibited the appropriate mineralogical and geochemical features, but also indicated that the secondary porosity provided by the fracture patterns was very small. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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28 pages, 6475 KiB  
Article
Valorization of Slags Produced by Smelting of Metallurgical Dusts and Lateritic Ore Fines in Manufacturing of Slag Cements
by Theofani Tzevelekou, Paraskevi Lampropoulou, Panagiota P. Giannakopoulou, Aikaterini Rogkala, Petros Koutsovitis, Nikolaos Koukouzas and Petros Petrounias
Appl. Sci. 2020, 10(13), 4670; https://doi.org/10.3390/app10134670 - 7 Jul 2020
Cited by 12 | Viewed by 3579
Abstract
A pyrometallurgical process was developed for the recycling of Ni bearing dusts and laterite ore fines by direct reduction smelting in DC (direct current) arc furnace. In the course of the performed industrial trials, besides the Ni-recovery in the liquid bath, slag composition [...] Read more.
A pyrometallurgical process was developed for the recycling of Ni bearing dusts and laterite ore fines by direct reduction smelting in DC (direct current) arc furnace. In the course of the performed industrial trials, besides the Ni-recovery in the liquid bath, slag composition was deliberately adjusted in order to produce a series of metallurgical slags with different chemical and mineralogical composition. The aim of this study was to investigate their suitability as clinker substitute in cement manufacturing. Examined parameters were slag FeOx content, basicity and applied cooling media (air, water cooling). A series of composite Portland and slag cements were manufactured in laboratory scale incorporating 20% and 40% of each slag, respectively; the rest being clinker of OPC (ordinary Portland cement) and 5% gypsum. The extended mineralogical analysis and microstructural properties of the produced slags were examined and correlated with the properties of the produced cements. The physical and mechanical characteristics of all examined cement products were found to meet the requirements of the regulation set for cements. The present research revealed that the most critical parameter in the compressive strength development of the slag cements is the mineralogical composition of the slag. Even in cases where rapid cooling to obtain glassy matrix is not feasible, adjustment of slag analysis to obtain mineralogical phases similar to those met in clinker of OPC, even at higher FeO contents (up to ~21wt.%), can result in production of slag with considerable latent hydraulic properties. These results indicate that there is potentially space for adjustments in conventional EAF (electric arc furnace) steel slags composition to allow for their wider use in cement manufacturing with significant environmental and economic benefits resulting from the reduction of energy requirements, CO2 emissions and natural raw materials consumption. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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10 pages, 2427 KiB  
Article
Role of Internal Stress in the Early-Stage Nucleation of Amorphous Calcium Carbonate Gels
by Qi Zhou, Tao Du, Lijie Guo, Gaurav Sant and Mathieu Bauchy
Appl. Sci. 2020, 10(12), 4359; https://doi.org/10.3390/app10124359 - 25 Jun 2020
Cited by 4 | Viewed by 2102
Abstract
Although calcium carbonate (CaCO3) precipitation plays an important role in nature, its mechanism remains only partially understood. Further understanding the atomic driving force behind the CaCO3 precipitation could be key to facilitate the capture, immobilization, and utilization of CO2 [...] Read more.
Although calcium carbonate (CaCO3) precipitation plays an important role in nature, its mechanism remains only partially understood. Further understanding the atomic driving force behind the CaCO3 precipitation could be key to facilitate the capture, immobilization, and utilization of CO2 by mineralization. Here, based on molecular dynamics simulations, we investigate the mechanism of the early-stage nucleation of an amorphous calcium carbonate gel. We show that the gelation reaction manifests itself by the formation of some calcium carbonate clusters that grow over time. Interestingly, we demonstrate that the gelation reaction is driven by the existence of some competing local molecular stresses within the Ca and C precursors, which progressively get released upon gelation. This internal molecular stress is found to originate from the significantly different local coordination environments exhibited by Ca and C atoms. These results highlight the key role played by the local stress acting within the atomic network in governing gelation reactions. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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16 pages, 3501 KiB  
Article
Numerical Prediction of the Behavior of CO2 Bubbles Leaked from Seafloor and Their Convection and Diffusion near Southeastern Coast of Korea
by Se-Min Jeong, Seokwon Ko and Wu-Yang Sean
Appl. Sci. 2020, 10(12), 4237; https://doi.org/10.3390/app10124237 - 20 Jun 2020
Cited by 6 | Viewed by 6799
Abstract
Among various carbon capture and storage technologies to mitigate global warming and ocean acidification due to greenhouse gases, ocean geological storage is considered the most feasible for Korea due to insufficient inland space to store CO2. However, the risk of CO [...] Read more.
Among various carbon capture and storage technologies to mitigate global warming and ocean acidification due to greenhouse gases, ocean geological storage is considered the most feasible for Korea due to insufficient inland space to store CO2. However, the risk of CO2 leakage and the behavior and environmental effects of the leaked CO2 need to be assessed for its successful implementation. Therefore, the behavior of CO2 bubbles/droplets dissolving into the surrounding seawater and the diffusion of dissolved CO2 by ocean flows should be accurately predicted. However, finding corresponding research has been difficult in Korea. Herein, the behavior and convection-diffusion of CO2 that was assumed to have leaked from the seafloor near the southeastern coast of Korea were numerically predicted using a multi-scale ocean model for the first time. In the simulation region, one of the pilot projects of CO2 ocean geological storage had started but has been temporarily halted. In the ocean model, hydrostatic approximation and the Eulerian–Lagrangian two-phase model were applied for meso- and small-scale regions, respectively. Parameters for the simulations were the leakage rate and the initial diameter of CO2. Results revealed that all leaked and rising CO2 bubbles were dissolved into the seawater before reaching the free surface; further, the change in the partial pressure of CO2 did not exceed 500 ppm during 30 days of leakage for all cases. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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14 pages, 4602 KiB  
Article
Durability and Mechanical Characteristics of Blast-Furnace Slag Based Activated Carbon-Capturing Concrete with Respect to Cement Content
by Seungwon Kim and Cheolwoo Park
Appl. Sci. 2020, 10(6), 2083; https://doi.org/10.3390/app10062083 - 19 Mar 2020
Cited by 4 | Viewed by 1936
Abstract
The recent abnormal temperature phenomena such as the rise of global mean temperature and sea level due to global climate change are clear threats that can no longer be overlooked to the human beings who have pursued indiscriminate development and rapid growth. Climate [...] Read more.
The recent abnormal temperature phenomena such as the rise of global mean temperature and sea level due to global climate change are clear threats that can no longer be overlooked to the human beings who have pursued indiscriminate development and rapid growth. Climate change has emerged as a serious risk that threatens the survival of the entire human race from the environmental and ecological aspects, despite international efforts for several decades. The CO2 concentration in the atmosphere has increased by approximately 39% since the industrial revolution. Even if carbon emissions are stopped right now, it is expected to take at least 50–200 years to return to the CO2 level before the industrial revolution. Therefore, we conducted an experimental study to develop a carbon-capturing concrete that has active as well as passive carbon reduction functions using blast-furnace slag, an industrial byproduct, instead of cement. For active carbon reduction, we used calcium hydroxide and sodium silicate as carbon capture activators, and conducted tests on mechanical properties and durability characteristics. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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13 pages, 1849 KiB  
Article
Large-Scale Screening and Machine Learning to Predict the Computation-Ready, Experimental Metal-Organic Frameworks for CO2 Capture from Air
by Xiaomei Deng, Wenyuan Yang, Shuhua Li, Hong Liang, Zenan Shi and Zhiwei Qiao
Appl. Sci. 2020, 10(2), 569; https://doi.org/10.3390/app10020569 - 13 Jan 2020
Cited by 44 | Viewed by 6556
Abstract
The rising level of CO2 in the atmosphere has attracted attention in recent years. The technique of capturing CO2 from higher CO2 concentrations, such as power plants, has been widely studied, but capturing lower concentrations of CO2 directly from [...] Read more.
The rising level of CO2 in the atmosphere has attracted attention in recent years. The technique of capturing CO2 from higher CO2 concentrations, such as power plants, has been widely studied, but capturing lower concentrations of CO2 directly from the air remains a challenge. This study uses high-throughput computer (Monte Carlo and molecular dynamics simulation) and machine learning (ML) to study 6013 computation-ready, experimental metal-organic frameworks (CoRE-MOFs) for CO2 adsorption and diffusion properties in the air with very low concentrations of CO2. First, the law influencing CO2 adsorption and diffusion in air is obtained as a structure-performance relationship, and then the law influencing the performance of CO2 adsorption and diffusion in air is further explored by four ML algorithms. Random forest (RF) was considered the optimal algorithm for prediction of CO2 selectivity, with an R value of 0.981, and this algorithm was further applied to analyze the relative importance of each metal-organic framework (MOF) descriptor quantitatively. Finally, 14 MOFs with the best properties were successfully screened out, and it was found that a key to capturing a low concentration CO2 from the air was the diffusion performance of CO2 in MOFs. When the pore-limiting diameter (PLD) of a MOF was closer to the CO2 dynamic diameter, this MOF could possess higher CO2 diffusion separation selectivity. This study could provide valuable guidance for the synthesis of new MOFs in experiments that capture directly low concentration CO2 from the air. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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19 pages, 4448 KiB  
Article
Comparative Kinetic Analysis of CaCO3/CaO Reaction System for Energy Storage and Carbon Capture
by Larissa Fedunik-Hofman, Alicia Bayon and Scott W. Donne
Appl. Sci. 2019, 9(21), 4601; https://doi.org/10.3390/app9214601 - 29 Oct 2019
Cited by 43 | Viewed by 10123
Abstract
The calcium carbonate looping cycle is an important reaction system for processes such as thermochemical energy storage and carbon capture technologies, which can be used to lower greenhouse gas emissions associated with the energy industry. Kinetic analysis of the reactions involved (calcination and [...] Read more.
The calcium carbonate looping cycle is an important reaction system for processes such as thermochemical energy storage and carbon capture technologies, which can be used to lower greenhouse gas emissions associated with the energy industry. Kinetic analysis of the reactions involved (calcination and carbonation) can be used to determine kinetic parameters (activation energy, pre-exponential factor, and the reaction model), which is useful to translate laboratory-scale studies to large-scale reactor conditions. A variety of methods are available and there is a lack of consensus on the kinetic parameters in published literature. In this paper, the calcination of synthesized CaCO3 is modeled using model-fitting methods under two different experimental atmospheres, including 100% CO2, which realistically reflects reactor conditions and is relatively unstudied kinetically. Results are compared with similar studies and model-free methods using a detailed, comparative methodology that has not been carried out previously. Under N2, an activation energy of 204 kJ mol−1 is obtained with the R2 (contracting area) geometric model, which is consistent with various model-fitting and isoconversional analyses. For experiments under CO2, much higher activation energies (up to 1220 kJ mol−1 with a first-order reaction model) are obtained, which has also been observed previously. The carbonation of synthesized CaO is modeled using an intrinsic chemical reaction rate model and an apparent model. Activation energies of 17.45 kJ mol−1 and 59.95 kJ mol−1 are obtained for the kinetic and diffusion control regions, respectively, which are on the lower bounds of literature results. The experimental conditions, material properties, and the kinetic method are found to strongly influence the kinetic parameters, and recommendations are provided for the analysis of both reactions. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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17 pages, 5297 KiB  
Article
An Experimental and Numerical Study of CO2–Brine-Synthetic Sandstone Interactions under High-Pressure (P)–Temperature (T) Reservoir Conditions
by Zhichao Yu, Siyu Yang, Keyu Liu, Qingong Zhuo and Leilei Yang
Appl. Sci. 2019, 9(16), 3354; https://doi.org/10.3390/app9163354 - 15 Aug 2019
Cited by 10 | Viewed by 2502
Abstract
The interaction between CO2 and rock during the process of CO2 capture and storage was investigated via reactions of CO2, formation water, and synthetic sandstone cores in a stainless-steel reactor under high pressure and temperature. Numerical modelling was also [...] Read more.
The interaction between CO2 and rock during the process of CO2 capture and storage was investigated via reactions of CO2, formation water, and synthetic sandstone cores in a stainless-steel reactor under high pressure and temperature. Numerical modelling was also undertaken, with results consistent with experimental outcomes. Both methods indicate that carbonates such as calcite and dolomite readily dissolve, whereas silicates such as quartz, K-feldspar, and albite do not. Core porosity did not change significantly after CO2 injection. No new minerals associated with CO2 injection were observed experimentally, although some quartz and kaolinite precipitated in the numerical modelling. Mineral dissolution is the dominant reaction at the beginning of CO2 injection. Results of experiments have verified the numerical outcomes, with experimentally derived kinetic parameters making the numerical modelling more reliable. The combination of experimental simulations and numerical modelling provides new insights into CO2 dissolution mechanisms in high-pressure/temperature reservoirs and improves understanding of geochemical reactions in CO2-brine-rock systems, with particular relevance to CO2 entry of the reservoir. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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20 pages, 5574 KiB  
Article
Carbon Spheres as CO2 Sorbents
by P. Staciwa, U. Narkiewicz, D. Sibera, D. Moszyński, R. J. Wróbel and R. D. Cormia
Appl. Sci. 2019, 9(16), 3349; https://doi.org/10.3390/app9163349 - 15 Aug 2019
Cited by 26 | Viewed by 3597
Abstract
Microporous nanocarbon spheres were prepared by using a microwave assisted solvothermal method. To improve the carbon dioxide adsorption properties, potassium oxalate monohydrate and ethylene diamine (EDA) were employed, and the influence of carbonization temperature on adsorption properties was investigated. For nanocarbon spheres containing [...] Read more.
Microporous nanocarbon spheres were prepared by using a microwave assisted solvothermal method. To improve the carbon dioxide adsorption properties, potassium oxalate monohydrate and ethylene diamine (EDA) were employed, and the influence of carbonization temperature on adsorption properties was investigated. For nanocarbon spheres containing not only activator, but also EDA, an increase in the carbonization temperature from 600 °C to 800 °C resulted in an increase of the specific surface area of nearly 300% (from 439 to 1614 m2/g) and an increase of the CO2 adsorption at 0 °C and 1 bar (from 3.51 to 6.21 mmol/g). Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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13 pages, 1638 KiB  
Article
Carbon Footprint of the Agricultural Sector in Qinghai Province, China
by Xiuhong Wang and Yili Zhang
Appl. Sci. 2019, 9(10), 2047; https://doi.org/10.3390/app9102047 - 17 May 2019
Cited by 8 | Viewed by 2355
Abstract
The agricultural sector has become an important emitter of greenhouse gases in China. The CO2 emissions in the western undeveloped region have attracted less attention than those in the eastern developed region in China. In this paper, the change in carbon footprint [...] Read more.
The agricultural sector has become an important emitter of greenhouse gases in China. The CO2 emissions in the western undeveloped region have attracted less attention than those in the eastern developed region in China. In this paper, the change in carbon footprint (CF) caused by agrochemical and agricultural energy inputs, the contributions of various inputs to the total carbon footprint (TCF), and the different changing trends between carbon intensity in output value (CV) and carbon intensity in area (CA) in Qinghai province were studied based on the data for agrochemical and energy inputs over 1995–2016. The change in TCF had a roughly stable period over 1995–1999, a slowly decreasing period over 2000–2007, and a rapidly increasing period over 2008–2016, which generally synchronize with the periods of before the Grain for Green Policy (GFGP), during the GFGP, and after the GFGP, respectively. The chemical nitrogen fertilizer and energy inputs were the principal factors influencing the TCF. The N fertilizer was the highest contributor to the TCF and contributed more to the relatively lower TCF during the GFGP in the study area. The relative CF caused by plastic film and diesel input in the study area increased faster than that in the whole country. The CV declined, with a mean of 0.022 kg carbon equivalent (CE)/Chinese Yuan (CNY), which was 55.59% of the mean CV in China over 1995–2016; inversely, the CA obviously rose after 2007, with a mean of 5.11 kg CE/ha, which was only 1.94% of the mean CA in China from 1995 to 2016. Compared with the whole country, Qinghai province generally had a higher rate of increase of carbon efficiency accompanied by a higher rate of increase of CA. The improvements of local agricultural activities should aim to keep a balance between higher carbon efficiency and lower CA in the study area. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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9 pages, 3512 KiB  
Article
Air Purification Performance of Photocatalytic Concrete Paving Blocks after Seven Years of Service
by Hubert Witkowski, Wioletta Jackiewicz-Rek, Karol Chilmon, Janusz Jarosławski, Anna Tryfon-Bojarska and Arkadiusz Gąsiński
Appl. Sci. 2019, 9(9), 1735; https://doi.org/10.3390/app9091735 - 26 Apr 2019
Cited by 18 | Viewed by 3645
Abstract
This paper presents the results of laboratory tests on photocatalytic pavement blocks from a bicycle lane in Poland after seven years of service. Air purification performance was tested on dusty and clean samples using different light sources and setups, with non-laminar gas circulation. [...] Read more.
This paper presents the results of laboratory tests on photocatalytic pavement blocks from a bicycle lane in Poland after seven years of service. Air purification performance was tested on dusty and clean samples using different light sources and setups, with non-laminar gas circulation. Secondary Electrons Secondary Ions (SESI) and InLens detectors combined with SEM–EDS and X-ray analyses were applied to confirm the presence of TiO2 in the studied blocks. The obtained results show that TiO2 was present in the form of agglomerates with a diameter of 0.25–5 µm and was bonded to the cement matrix components. The tested samples still maintained nitric oxide (NO) removal capability with a NO reduction rate of 4–45%, depending on light source and surface cleanliness. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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30 pages, 5860 KiB  
Article
Soil-Gas Concentrations and Flux Monitoring at the Lacq-Rousse CO2-Geological Storage Pilot Site (French Pyrenean Foreland): From Pre-Injection to Post-Injection
by Frédérick Gal, Zbigniew Pokryszka, Nadège Labat, Karine Michel, Stéphane Lafortune and André Marblé
Appl. Sci. 2019, 9(4), 645; https://doi.org/10.3390/app9040645 - 14 Feb 2019
Cited by 21 | Viewed by 4194
Abstract
Soil-gas concentrations and flux were measured during 20 separate measurement campaigns at the TOTAL Lacq-Rousse carbon capture and storage (CCS) pilot site, southern France, where 51,000 tons of CO2 were injected in a depleted natural gas field. Baseline data (September 2008 to [...] Read more.
Soil-gas concentrations and flux were measured during 20 separate measurement campaigns at the TOTAL Lacq-Rousse carbon capture and storage (CCS) pilot site, southern France, where 51,000 tons of CO2 were injected in a depleted natural gas field. Baseline data (September 2008 to December 2009) are compared to monitoring data from the injection (March 2010 to March 2013) and post-injection (February 2014 to December 2015) periods. CO2 soil-gas concentrations varied from atmospheric concentrations to more than 16% vol. with 1.4% as median value. Summer data showed high CO2 concentrations in the soil that remained quite high during winter. Median CO2 flux at the soil/atmosphere interface was close to 4.4 cm3·min−1·m−2. Carbon-isotope ratios measured on CO2 in soil gas had a mean value of −23.5 ± 3.1‰, some deviation being due to atmospheric CO2. Comparison between different gas species and the influence of temperature, pressure and soil-water content suggest that gases in near-surface environments are produced locally and naturally, and are unrelated to CO2 ascending from the storage reservoir. Monitoring of CO2 injection and the use of threshold levels is discussed as part of a practical approach considering specific regulations for the Lacq-Rousse CCS pilot experiment and constraints for the site operator. Full article
(This article belongs to the Special Issue Climate Change, Carbon Capture, Storage and CO2 Mineralisation Technologies)
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